Stability of single-atom catalysts for electrocatalysis

Hu, Hao; Wang, Jiale; Tao, Peng; Song, Chengyi; Shang, Wen; Deng, Tao; Wu, Jianbo

doi:10.1039/d1ta08582d

Cited by 65 publications

(42 citation statements)

References 123 publications

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“…87 They may loss the active sites due to demetalation and carbon oxidation (two main degradation mechanisms) at high potentials and should be carefully considered for practical catalyst design. 88 Besides, the coordination environment for SACs and DACs is still limited, 27,34,63,89,90 and more stable support materials with suitable anchoring points are thus highly desirable to further enrich the family.…”

Section: Discussionmentioning

confidence: 99%

“…In addition, the stability of SACs is another important issue to be addressed prior to their practical applications in electrocatalysis. 27…”

Section: Introductionmentioning

confidence: 99%

“…In addition, the stability of SACs is another important issue to be addressed prior to their practical applications in electrocatalysis. 27 As a natural extension of SACs, dual-atom catalysts (DACs) containing various dispersed metal dimers have attracted great attention in recent years. [28][29][30][31][32][33][34][35][36] Their high metal loading and more exible catalytically active sites bring about rich synergistic effects, which could fundamentally break the linear scaling relationships between various intermediates to achieve superior catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Dual-metal atom incorporated N-doped graphenes as oxygen evolution reaction electrocatalysts: high activities achieved by site synergies

Zhang

Qin

et al. 2022

J. Mater. Chem. A

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Section: Discussionmentioning

confidence: 99%

“…In addition, the stability of SACs is another important issue to be addressed prior to their practical applications in electrocatalysis. 27…”

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Dual-metal atom incorporated N-doped graphenes as oxygen evolution reaction electrocatalysts: high activities achieved by site synergies

Zhang

Qin

et al. 2022

J. Mater. Chem. A

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“…As a new frontier catalytic material, supported single-atom catalysts (SACs) have attracted extensive attention in the recent decade since the concept of “single-atom catalysis” was first introduced by Zhang et al With the high atom utilization and remarkable catalytic activity, SACs exhibit great potential for applications for electrochemical energy conversion and storage processes, such as hydrogen evolution reaction (HER), oxygen evolution reaction (OER), carbon dioxide reduction (CO 2 RR), , nitrogen reduction reaction (NRR), , oxygen reduction reaction (ORR), − etc. Despite numerous studies focusing on the design, synthesis, and application of SACs, their commercialization is still limited due to the pursuit of better activity and selectivity at the expense of stability, which is a more critical factor hindering large-scale applications. − …”

Section: Introductionmentioning

confidence: 99%

Dynamic Stability of Copper Single-Atom Catalysts under Working Conditions

et al. 2022

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The long-term stability of single-atom catalysts is a major factor affecting their large-scale commercial application. How to evaluate the dynamic stability of single-atom catalysts under working conditions is still lacking. Here, taking a single copper atom embedded in N-doped graphene as an example, the "constant-potential hybrid-solvation dynamic model" is used to evaluate the reversible transformation between copper single atoms and clusters under realistic reaction conditions. It is revealed that the adsorption of H is a vital driving force for the leaching of the Cu single atom from the catalyst surface. The more negative the electrode potential, the stronger the adsorption of H. As a result, the competitive hydrogen evolution reaction is inhibited, and Cu−N bonds are weakened, resulting in some Cu atoms being tethered on the catalyst surface and some being dissolved in the aqueous solution. The collision of the Cu atoms in the two states forms a transient Cu cluster structure as a true catalytic active site to promote CO 2 reduction to ethanol. As the applied potential is released or switched to a positive value, hydroxyl radicals (OH • ) play a dominant role in the oxidation process of the Cu cluster, and then Cu returns to the initial atomic dispersion state by redeposition, completing the reconstruction cycle of the copper catalyst. Our work provides a fundamental understanding of the dynamic stability of Cu single-atom catalysts under working conditions at the atomic level and calls for a reassessment of the stability of currently reported single-atom catalysts considering realistic reaction conditions.

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“…The creation of two neighboring functional groups upon plasma treatment at well-defined positions in the BL allows the possibility of its application as a model system for the anchoring of different TMs in the study of the fundamental properties of SACs. Thus, important aspects such as long-term stability under harsh (thermal 34 and electrochemical 35 ) reaction conditions and local electronic and geometric effects can be tackled in a controlled environment. Our bifunctionalization approach represents the first steps into the development of a new type of model system offering coexisting chemically different active sites with a well-defined structure and position, aiming at the fundamental understanding of the properties mentioned above, as well as possible confinement 36 and synergistic 37 effects.…”

Section: ■ Introductionmentioning

confidence: 99%

Plasma Functionalization of Silica Bilayer Polymorphs

Prieto

Mullan

Wan

et al. 2022

ACS Appl. Mater. Interfaces

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Ultrathin silica films are considered suitable two-dimensional model systems for the study of fundamental chemical and physical properties of all-silica zeolites and their derivatives, as well as novel supports for the stabilization of single atoms. In the present work, we report the creation of a new model catalytic support based on the surface functionalization of different silica bilayer (BL) polymorphs with well-defined atomic structures. The functionalization is carried out by means of in situ H-plasma treatments at room temperature. Low energy electron diffraction and microscopy data indicate that the atomic structure of the films remains unchanged upon treatment. Comparing the experimental results (photoemission and infrared absorption spectra) with density functional theory simulations shows that H2 is added via the heterolytic dissociation of an interlayer Si–O–Si siloxane bond and the subsequent formation of a hydroxyl and a hydride group in the top and bottom layers of the silica film, respectively. Functionalization of the silica films constitutes the first step into the development of a new type of model system of single-atom catalysts where metal atoms with different affinities for the functional groups can be anchored in the SiO2 matrix in well-established positions. In this way, synergistic and confinement effects between the active centers can be studied in a controlled manner.

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Stability of single-atom catalysts for electrocatalysis

Abstract: Single-atom catalysts (SACs) have attracted significant attention in recent years for their maximum atomic utilization and high efficiency in a series of electrocatalytic reactions. However, the atomic-dispersed metal atoms have...

Cited by 65 publications

References 123 publications

Dual-metal atom incorporated N-doped graphenes as oxygen evolution reaction electrocatalysts: high activities achieved by site synergies

Dual-metal atom incorporated N-doped graphenes as oxygen evolution reaction electrocatalysts: high activities achieved by site synergies

Dynamic Stability of Copper Single-Atom Catalysts under Working Conditions

Plasma Functionalization of Silica Bilayer Polymorphs

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